Contamination and health risk of phthalate esters in soils from a typical waste plastic recycling area

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1 ENVIRONMENTAL CHEMISTRY Vol 35 No 2 February 2016 DOI /j issn J WANG Yuwen CHAI Miao ZENG Ning et al Contamination and health risk of phthalate esters in soils from a typical waste plastic recycling area J Environmental Chemistry * ** PAEs μg g μg g - 1 PAEs DEHP DIBP DBP PAEs DEHP 68 8% PAEs EPA 6 PAEs 2- DEHP PAEs Contamination and health risk of phthalate esters in soils from a typical waste plastic recycling area WANG Yuwen 1 CHAI Miao 1 ZENG Ning 2 TANG Zhenwu 1** 1 Environmental Research Academy North China Electric Power University Beijing China 2 Institute of Materials China Academy of Engineering Physics Mianyang China Abstract Levels and distributions of phthalate esters PAEs were investigated in surface soils from a typical waste plastic recycling area in Hebei China The results showed that the concentrations of total PAEs ranged from to 30 1 μg g - 1 with a mean value of 6 98 μg g - 1 Levels of PAEs in the investigated soils were similar to those soils in some e-waste recycling areas and were one to two orders of magnitude higher than those reported in other urban soils from China Di 2-ethylhexyl phthalate DEHP was the dominant congener representing 68 8% of the total PAEs in the study soils followed by diisobutyl phthalate DIBP and dibutyl phthalate DBP Source assessment indicated that the emission from waste plastic recycling was a major contributor to PAEs in the soils The carcinogenic and non-carcinogenic risks of six congeners i e dimethyl phthalate diethyl phthalate dibutyl phthalate benzyl butyl phthalate di 2-ethylhexyl phthalate and di-n-octylophthalate classed as priority pollutants by US EPA and European Union were estimated Received July * MS60 Supported by the National Environmental Protection Public Welfare Science and Technology Research Program of China and the Fundamental Research Funds for the Central Universities 2015MS60 ** Tel zwtang@ ncepu edu cn Corresponding author Tel zwtang@ ncepu edu cn

2 2 365 through the main pathways ingestion inhalation and dermal contact The non-carcinogenic risks to adults and children from exposure to soil DEHP exceeded the acceptable level Our results show that crude plastic waste processing is a major contributor to PAEs in the soils which should be of great concern Keywords waste plastic recycling soils phthalate esters PAEs distribution health risks Phthalate esters PAEs 1 PAEs PAEs PAEs PAEs PAEs PAEs 4-14 PAEs PAEs PAEs PAEs 1 Materials and methods HJ km 1 # 17 # 18 # 22 # 23 # 27 # 28 # 29 # 30 # 2 # 7 # 10 # 14 # 16 # 20 # 24 # 3 # 4 # 5 # 6 # 8 # 9 # 11 # 12 # 13 # 15 # 19 # 21 # 25 # 26 # cm 10 m kg < DMP DEP DIBP DBP 2- DMEP BMPP 2- DEEP DPP DHXP BBP 2- DBEP DCHP 2- DEHP DPHP DNOP DNP AccuStandard J K Baker KX-2013TD 360 W 40 khz RE52CS-1 D10 12

3 V V = min h h3% h 10 mm350 mm 1 cm 4 cm 1 cm 40 ml g 50 ml 30 ml / V V = min 3 g 5 g 100 ml 30 ml 2 20 min 2 ml 70 ml / V V = ml 0 50 ml GC /MS Agilent7890GC /5975MS HP - 5MS 30 m 0 25 mm 0 25 μm min20 min min 5 min min % 1 0 ml min NCI MS min amu SIM 1 5 PAEs PAEs μg L PAEs 84 7% 123 2% DMP DEP DIBP DBP DMEP BMPP DEEP DPP DHXP BBP DBEP DCHP DEHP DPHP DNOP DNP μg kg - 1 Fig 1 1 Location of soil sampling sites

4 USEPA PAEs PAEs DMP DEP DBP DNOP DEHP BBP PAEs ADD intake = C soil BAF IRF EF ED CF BW AT ADD ingest = C soil IRS EF ED CF BW AT ADD demal = C soil SA AF ABS EF ED CF BW AT ADD inhale = C soil EF ED I j PEF AT CR = ADD i CFS HQ = ADD i RfD i C soil mg kg - 1 ADD i mg kg - 1 day - 1 HQ CR 1 Parameter Meaning Table Parameters for risk assessment in this study Unit Adults Numerical data Children Source IRS mg d AF mg cm SA cm 2 d ED a BW kg IRF mg d EF d a CF PEF m 3 kg I j m 3 d CFS mg kg - 1 d DEHP BBP ABS AT d RfD BAF 365 ED DMP 10 DEP 0 8 mg kg - 1 d - 1 DBP BBP 0 2 DEHP 0 02 DNOP 0 04 DEP PAEs DBP DEHP DNOP 0 166

5 HQ > 1 CR > Results and discussion 2 1 PAEs 16 PAEs 16 PAEs μg g μg g μg g DEHP μg g μg g μg g PAEs μg g - 1 PAEs PAEs P > # 16 PAEs 10 # PAEs 23# 15 Fig 2 2 PAEs Levels of PAEs in the soils from waste plastic recycling PAEs 2 Table 2 2 PAEs Phthalate ester PAE concentrations in soil samples from the waste plastic recycling area and other areas Location Time DEHP Concentration of DEHP / μg g - 1 PAEs Concentration of PAEs / μg g - 1 Homologs number Reference ND ND ND ND PAEs 1 1

6 PAEs 10 0 μg g % 20 DBP μg g μg g - 1 DEHP PAEs DBP μg g - 1 DEHP 4 35 μg g - 1 PAEs 2 2 PAEs 16 DCHP 10% 100% 3 DEHP 4 42% 97 1% 68 8% 77 0% DIBP DBP 16 PAEs 12 9% 3 43% DEHP DIBP DBP 85 1% DEHP DIBP DBP PAEs 25 DEHP K ow log K ow DEHP Fig 3 3 PAEs Congener patterns of PAEs in soils from waste plastic recycling sites 2 3 PAEs PAEs 30 PVC 31 70% 32 PAEs % 4 Fig 4 4 PAEs Factor loadings of PAE congeners on two principal components analysis PC1 57 0% DEP DMP BBP DNOP DNP DPP DMEP r DBP BBP DEP DEHP DNOP PVC PVC

7 PVC PC2 22 6% DCHP DBEP DPHP r P 0 DPHP DBEP DCHP DBEP DCHP PC3 8 03% DEHP DBP DEHP DBP 24 PAEs 2 4 PAEs EPA 6 PAEs 6 BBP DEHP DEP DMP DBP BBP DNOP % DEHP 6 PAEs HQ % DEHP 6 PAEs HQ 1 0 DEHP 6 PAEs DEHP BBP 3 DEHP CR EPA BBP CR DEHP BBP DEHP DEHP DEHP DEHP Table 3 Range 3 DEHP BBP Carcinogenic risks CR of DEHP and BBP to adults and children Adults Average % 95% confidence interval upper limit Range Children Average % 95% confidence interval upper limit PAEs PAEs 11 0% 75 1% 38 PAEs PBDEs 3 Conclusion PAEs 1 2 PAEs DBP DEHP PAEs DEHP 6 PAEs DEHP DEHP DIBP DBP PAEs PAEs

8 2 371 References J WU H Q ZHU Z X HUANG X L et al Study on determination of 21 phthalate acid esters and their distributions in different types of foods by Gas Chromatography-Mass Spectrometry J Journal of Instrumental Analysis in Chinese 2 J WANG L X YANG X Research advance on toxicity and health effect of phthalate review and perspective J J Environ Health in Chinese 3 J CHEN B NI J Toxicity and health effect of phthalate acid esters J Technology & Development of Chemical Industry in Chinese 4 J LIU W L ZHANG Z ZHU L Q et al Distribution characteristics of phthalic acid esters in soils and plantsate-waste recycling sites in Taizhou of Zhejiang China J Chinese Journal of Applied Ecology in Chinese 5 D 2009 CHU H B PAHs and PAEs in leachates waters and soils around landfill sites in Guangzhou city D Guangzhou Guangzhou university 2009 in Chinese 6 J XIONG P X GONG X DENG L Analysis of PAE pollutants in farm soil and water samples in Nanchang city J Chemsitry Online in Chinese 7 LI X H Ma L L Liu X F et al Phthalate ester pollution in urban soil of Beijing People's Republic of China J Bull Environ Contam Toxicol ZENG F Cui K Y Xie Z Y et al Distribution of phthalate esters in urban soils of subtropical city Guangzhou China J J Hazard Mater ZENG F Cui K Y Xie Z Y et al Phthalate esters PAEs Emerging organic contaminants in agricultural soils in peri-urban areas around Guangzhou China J Environ Pollut MA T T Wu L H Chen L et al Phthalate esters contamination in soils and vegetables of plastic film greenhouses of suburb Nanjing China and the potential human health risk J Environ Sci Pollut Res ZHANG Y Wang P J Wang L et al The influence of facility agriculture production on phthalate esters distribution in black soils of northeast China J Sci Total Environ GIBSON R WANG M J PADGETT E et al Analysis of 4-nonylphenols phthalates and polychlorinated biphenyls in soils and blosolids J Chemosphere PEIJNENBURG W J G M STRUIJS J Occurrence of phthalate esters in the environment of the Netherlands J Ecotoxicol Environ Saf VIKELS E J THOMSEN M CARLSEN L Phthalates and nonylphenols in profiles of differently dressed soils J Sci Total Environ TANG Z W Huang Q F Cheng J L et al Polybrominated diphenyl ethers in soils sediments and human hair in a plastic waste recycling area a neglected heavily polluted area J Environ Sci Technol US EPA United States Environmental Protection Agency 2013 Mid Atlantic Risk Assessment Regional Screening Level RSL Summary Table S Washington DC 17 J WANG Y J LI J G XU W L et al Village resident nourishment of Hebei investigates with health condition J Journal of Hygiene Research in Chinese 18 WANG J Chen G C Christie P et al Occurrence and risk assessment of phthalate esters PAEs in vegetables and soils of suburban plastic film greenhouses J Sci Total Environ NMED New Mexico Environment Department 2009 Technical background document for development of soil screening levels S 20 MO C H Cai Q Y Tang SR et al Polycyclic aromatic hydrocarbons and phthalic acid esters in vegetables from nine farms of the Pearl River Delta South China J Arch Environ Contam Toxicol D 2014 LI T Pollution levels and risk assessment of 6 priority phthalate esters in water and sediments from estuaries of the Pearl River Delta D Guangzhou Jinan University 2014 in Chinese 22 WANG W Wu F Y Huang M J et al Size fraction effect on phthalate esters accumulation bioaccessibility and in vitro cytotoxicity of indoor /outdoor dust and risk assessment of human exposure J J Hazard Mater

9 LIU X W Shi J H Bo T et al Occurrence and risk assessment of selected phthalates in drinking water from waterworks in China J Environ Sci Pollut Res NIU L L Xu Y Xu C et al Status of phthalate esters contamination in agricultural soils across China and associated health risks J Environ Pollut Net S Sempéré R Delmont A et al Occurrence fate behavior and ecotoxicological state of phthalates in different environmental matrices J Environ Sci Technol DEHP J XIE Q S WANG S S CAI F Y et al Study on exposure level in environment media human body loading and toxic effects of Di 2- ethylhexy1 phthalate J J of Pub Health and Prev Med in Chinese 27 D 2002 XIA F Y Biodegradability research of phthalic acid esters D Hangzhou Zhejiang university 2002 in Chinese 28 / K OW K OC J PIAO H S TAO P HU H Y et al Sorption coefficient of organic compounds K OC were estimated according to the octanol / water partition coefficient K OW J Environmental Science and Technology in Chinese 29 DEHP D 2011 WANG J W Concentrations and risk assessment of DEHP vegetables around plastic industrial area D Hangzhou Zhejiang Gongshang University 2011 in Chinese 30 J ZHOU C YOU M Y LIU J Y et al The Source Analysis and Prevention Measures of Phthalate esters in edible oil J Journal of the Chinese Cereals and Oils Association in Chinese 31 J WU Z Y ZHU Y LI W et al Fast screening of phthalates in plastic products J Plastics Science and Technology in Chinese 32 J LI Z B CAI C L LIU X M Research progress in synthesis and application of phthalate plasticizers J Plastics Additives in Chinese 33 PVC 6 J WANG C Y ZHANG S W ZHANG Y W Simultaneous determination of six kinds of restricted phthalates in PVC toys and childcare articles J Polyvinyl Chloride in Chinese 34 PVC J / XU Y XIONG Y GUO S Y Issues caused by migration of plasticizers from flexible PVC and its countermeasures J Progress In Chemistry / in Chinese 35 J TANG G L HU B KANG Z L et al Situation and Problems of waste plastics recycling J Renewable Resources and Recycling Economy in Chinese 36 J JIANG P P FANG H X WEI L J et al Current situation and development trend of plasticizer for PVC J Polyvinyl Chloride in Chinese 37 EB /OL http / /www cnchemadd com /isoc - zl /shownews asp id = J YU Y J YE H YANG Y et al The bioaccessibility and exposure assessment of PAEs via oral media in Taihu Lake Basin of south Jiangsu province J Environmental Chemistry in Chinese

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